Synthesis of Hierarchical Copper-Containing Silicas under Near Neutral Conditions and Their Catalytic Properties in Phenol Hydroxylation

Copper-containing mesoporous silicas with different mesostructures were synthesized by co-condensation of tetramethoxysilane and Cu(APTES)42+ (APTES: (EtO)3Si(CH2)3NH2) with predefined copper species using P123 as template and KCl as additive under near neutral conditions. Scanning electron microscopy and nitrogen adsorption characterization showed that the material with a hierarchical pore structure was obtained at high Cu(APTES)42+/TMOS ratio. In phenol hydroxylation using H2O2 as oxidant, the material with the hierarchical porous structure showed a higher catalytic activity than that with only the mesoporous structure.

摘要：在近中性条件下, 以正硅酸甲酯和 Cu(APTES)42+ (APTES: (EtO)3Si(CH2)3NH2) 为前驱体, P123 为模板剂, KCl 为添加剂合成了不同孔结构的含铜介孔氧化硅材料. 扫描电镜和氮气吸附结果表明, 当 Cu(APTES)42+/TMOS 摩尔比较高时能得到具有多级孔结构的材料. 在以 H2O2 为氧化剂的苯酚羟基化反应中, 具有多级孔结构的含铜介孔氧化硅材料表现出比单一介孔材料高的催化性能.

Graphical abstractCopper-containing mesoporous silicas with hierarchical porosity were synthesized under near neutral conditions. This kind of material shows higher catalytic activity than that with only mesopores for the hydroxylation of phenol using H2O2 as oxidant.Figure optionsDownload full-size imageDownload as PowerPoint slide